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The U.S. Environmental Protection Agency (EPA) presently uses a 40 ppbv background O3 level as a baseline in its O3 risk assessments. This background is defined as those concentrations that would exist in the absence of North American emissions. Lefohn et al. [2001] have argued that frequent occurrences of O3 concentrations above 50–60 ppbv at remote northern U.S. sites in spring are of stratospheric origin, challenging the EPA background estimate and implying that the current O3 standard (84 ppbv, 8-hour average) may be unattainable. We show that a 3-D global model of tropospheric chemistry reproduces much of the observed variability in U.S. surface O3 concentrations, including the springtime high-O3 events, with only a minor stratospheric contribution (always 2 km). It declines from spring to summer and further decreases during O3 pollution episodes. The 40 ppbv background assumed by EPA thus actually underestimates the risk associated with O3 during polluted conditions. A better definition would represent background as a function of season, altitude, and total surface O3 concentration. Natural O3 levels are typically 10–25 ppbv and never exceed 40 ppbv. International controls to reduce the hemispheric pollution background would facilitate compliance with an AOT40-type standard (cumulative exposure to O3 above 40 ppbv) in the United States.

An updated version of the nested-grid GEOS-Chem model is developed allowing for higher horizontal (0.5°×0.667°) resolution as compared to global models. CO transport over a heavily polluted region, the Beijing-Tianjin-Hebei (BTH) city cluster in China, and the pattern of outflow from East China in summertime are investigated. Comparison of the nested-grid with global models indicates that the fine-resolution nested-grid model is capable of resolving individual cities with high associated emission intensities. The nested-grid model indicates the presence of a high CO column density over the Sichuan Basin in summer, attributable to the low-level stationary vortex associated with the Basin's topographical features. The nested-grid model provides good agreement also with measurements from a suburban monitoring site in Beijing during summer 2005. Tagged CO simulation results suggest that regional emissions make significant contributions to elevated CO levels over Beijing on polluted days and that the southeastward moving cyclones bringing northwest winds to Beijing are the key meteorological mechanisms responsible for dispersion of pollution over Beijing in summer. Overall CO fluxes to the NW Pacific from Asia are found to decrease by a factor of 3–4 from spring to summer. Much of the seasonal change is driven by decreasing fluxes from India and Southeast Asia in summer, while fluxes from East China are only 30% lower in summer than in spring. Compared to spring, summertime outflow from Chinese source regions is strongest at higher latitudes (north of 35° N). The deeper convection in summer transporting CO to higher altitudes where export is more efficient is largely responsible for enhanced export in summer.

We use aircraft observations of carbon monoxide (CO) from the NASA ARCTAS and NOAA ARCPAC campaigns in April 2008 together with multiyear (2003–2008) CO satellite data from the AIRS instrument and a global chemical transport model (GEOS-Chem) to better understand the sources, transport, and interannual variability of pollution in the Arctic in spring. Model simulation of the aircraft data gives best estimates of CO emissions in April 2008 of 26 Tg month−1 for Asian anthropogenic, 9.4 for European anthropogenic, 4.1 for North American anthropogenic, 15 for Russian biomass burning (anomalously large that year), and 23 for Southeast Asian biomass burning. We find that Asian anthropogenic emissions are the dominant source of Arctic CO pollution everywhere except in surface air where European anthropogenic emissions are of similar importance. Russian biomass burning makes little contribution to mean CO (reflecting the long CO lifetime) but makes a large contribution to CO variability in the form of combustion plumes. Analysis of two pollution events sampled by the aircraft demonstrates that AIRS can successfully observe pollution transport to the Arctic in the mid-troposphere. The 2003–2008 record of CO from AIRS shows that interannual variability averaged over the Arctic cap is very small. AIRS CO columns over Alaska are highly correlated with the Ocean Niño Index, suggesting a link between El Niño and Asian pollution transport to the Arctic. AIRS shows lower-than-average CO columns over Alaska during April 2008, despite the Russian fires, due to a weakened Aleutian Low hindering transport from Asia and associated with the moderate 2007–2008 La Niña. This suggests that Asian pollution influence over the Arctic may be particularly large under strong El Niño conditions.

We examine the transatlantic transport of anthropogenic ozone and its impact on surface ozone in Europe and North America by using a 5-year (1993–1997) simulation with the GEOS-CHEM global three-dimensional model of tropospheric chemistry. Long-term time series of ozone and CO at Mace Head (Ireland) and Sable Island (Canada) are used to evaluate transatlantic transport in the model. North American anthropogenic emissions contribute on average 5 ppbv to surface ozone at Mace Head, and up to 10–20 ppbv during transatlantic transport events, which are forerunners of broader events in Europe. These events are associated with low-level westerly flow driven by an intense Icelandic low between Iceland and the British Isles. North American influence on ozone at Mace Head is strongly correlated with the North Atlantic Oscillation (NAO), implying that the NAO index can be used to forecast transatlantic transport of North American pollution to Europe. European anthropogenic emissions contribute on average less than 2 ppbv to surface ozone at Sable Island but up to 5–10 ppbv during transatlantic transport events. These events are associated with low-level easterly flow established by anomalous low pressure at 45°N over the North Atlantic. North American anthropogenic emissions enhance surface ozone in continental Europe by 2–4 ppbv on average in summer and by 5–10 ppbv during transatlantic transport events; transport in the boundary layer and subsidence from the free troposphere are both important mechanisms. We find in the model that 20% of the violations of the European Council ozone standard (55 ppbv, 8-hour average) in the summer of 1997 over Europe would not have occurred in the absence of anthropogenic emissions from North America. North American influence on surface ozone in Europe is particularly strong at the thresholds used for the European standards (55–65 ppbv).

We have conducted an observing system simulation experiment for the Tropospheric Emission Spectrometer (TES) satellite instrument to determine the potential of nadir retrievals of carbon monoxide (CO) from this instrument to constrain estimates of continental sources of CO. We use the GEOS-CHEM global chemical transport model to produce a pseudoatmosphere in which the relationship between sources and concentrations of CO is known. Linear profile retrievals of CO are calculated by sampling this pseudoatmosphere along the orbit of TES. These retrievals are used as pseudo-observations with a maximum a posteriori inverse algorithm to estimate the CO sources from the different continents. This algorithm accounts for the finite vertical resolution of the retrieval, instrument errors, and representation and transport errors in the GEOS-CHEM simulation of CO. The structure of the transport error is estimated using the statistics of the difference between paired GEOS-CHEM forecasts of CO, and this structure is then scaled to match the model error in the GEOS-CHEM simulation of aircraft observations of Asian outflow over the NW Pacific. We show that with proper characterization of observation errors just 2 weeks of observations from TES have the potential to constrain estimates of continental sources of CO to within 10%.